First principles characterization of spinterfaces between magnetic Cobaltocene molecule and 2D magnets (CrI$_3$, Fe$_3$GeTe$_2$)

TL;DR

This study uses first-principles calculations to analyze the electronic and magnetic properties of interfaces between cobaltocene molecules and 2D magnetic materials, revealing strong hybridization, anisotropic exchange interactions, and potential for spin-transport applications.

Contribution

It provides a detailed first-principles characterization of spinterfaces between cobaltocene and 2D magnets, highlighting hybridization, exchange mechanisms, and enhanced magnetic interactions.

Findings

Hybridization of electronic states across interfaces.

Strong directional anisotropy in magnetic interactions.

100% spin polarization at the Fermi level in Cobaltocene/CrI3 interface.

Abstract

In this paper, we examine the properties of spin-polarized interfaces consisting of single-molecule magnet bis(cyclopentadienyl)cobalt(II) (cobaltocene) and two-dimensional magnetic materials, semiconducting CrI$_3$ and metallic Fe$_3$GeTe$_2$, using first-principles density functional theory based calculations. Our calculated adsorption energies indicate the stability of these hetero-interfaces with the observation of hybridization of electronic states across the interface. Magnetic exchange interaction parameters have been obtained from both total energy differences and the Liechtenstein-Katsnelson-Antropov-Gubanov (LKAG) formalism in the basis of maximally localized Wannier functions (MLWFs). Analysis of these parameters shows a strong directional anisotropy in the magnetic substrate-molecule interaction in agreement with the nature of orbital hybridization. Additionally, possible exchange mechanisms are proposed based on orbital-resolved exchange and hopping parameters. We also show that the molecular adsorption may enhance the intralayer exchange interactions, with some exchange parameters reaching up to a 3-fold increase in magnitude compared to the freestanding case. Finally, we observe a 100 % spin polarization at the Fermi level in the cobaltocene/CrI$_3$ interface, which makes it particularly promising for spin-transport applications.